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Room-Temperature Chemoselective Hydrogenation of Nitroarene Over Atomic Metal-Nonmetal Catalytic Pair.

Jie DingFuhua LiJincheng ZhangHaifeng QiZhiming WeiChenliang SuHong Bin YangYueming ZhaiBin Liu
Published in: Advanced materials (Deerfield Beach, Fla.) (2023)
Constructing atomic catalytic pair emerges as an attractive strategy to achieve better catalytic performance. Herein, we report an atomic Ir 1 -P 1 /NPG catalyst with asymmetric Ir-N 2 P 1 sites that delivers superb activity and selectivity for hydrogenation of various functionalized nitrostyrene. In the hydrogenation reaction of 3-nitrostyrene, Ir 1 -P 1 /NPG (NPG refers to N,P-codoped graphene) shows a turnover frequency (TOF) of 1197 h -1 , while the reaction cannot occur over Ir 1 /NG (NG refers to N-doped graphene). Compared to Ir 1 /NG, the charge density of Ir site in Ir 1 -P 1 /NPG is greatly elevated, which is conducive to H 2 dissociation. Moreover, revealed by density functional theory (DFT) calculations and poisoning experiments, the P site in Ir 1 -P 1 /NPG is found able to bind nitrostyrene, while the neighboring Ir site provides H to reduce the nitro group in chemoselective hydrogenation of nitrostyrene. This work offers a successful example of establishing atomic catalytic pair for driving important chemical reactions, paving the way for the development of more advanced catalysts to further improve the catalytic performance. This article is protected by copyright. All rights reserved.
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